The response of hard-limiting bandpass limiters to PM signals
Hard limiting bandpass limiter output signal to noise ratio in PM signal detection calculated using probability density function
Chang, J. C.↗
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Theoretical Chemistry At NASA Ames Research Center
The theoretical work being carried out in the Computational Chemistry Branch at NASA Ames will be overviewed. This overview will be followed by a more in-depth discussion of our theoretical work to determine molecular opacities for the TiO and water molecules and a discussion of our density function theory (DFT) calculations to determine the harmonic frequencies and intensities to the vibrational bands of polycyclic aromatic hydrocarbons (PAHs) to assess their role as carriers to the unidentified infrared (UIR) bands. Finally, a more in-depth discussion of our work in the area of computational molecular nanotechnology will be presented.
Langhoff, Stephen↗
Formation of Carbon Nanotube Based Gears: Quantum Chemistry and Molecular Mechanics Study of the Electrophilic Addition of o-Benzyne to Fullerenes, Graphene, and Nanotubes
Considerable progress has been made in recent years in chemical functionalization of fullerene molecules. In some cases, the predominant reaction products are different from those obtained (using the same reactants) from polycyclic aromatic hydrocarbons (PAHs). One such example is the cycloaddition of o-benzyne to C60. It is well established that benzyne adds across one of the rings in naphthalene, anthracene and other PAHs forming the [2+4] cycloaddition product (benzobicyclo[2.2.2.]-octatriene with naphthalene and triptycene with anthracene). However, Hoke et al demonstrated that the only reaction path for o-benzyne with C60 leads to the [2+2] cycloaddition product in which benzyne adds across one of the interpentagonal bonds (forming a cyclobutene ring in the process). Either reaction product results in a loss of aromaticity and distortion of the PAH or fullerene substrate, and in a loss of strain in the benzyne. It is not clear, however, why different products are preferred in these cases. In the current paper, we consider the stability of benzyne-nanotube adducts and the ability of Brenner's potential energy model to describe the structure and stability of these adducts. The Brenner potential has been widely used for describing diamondoid and graphitic carbon. Recently it has also been used for molecular mechanics and molecular dynamics simulations of fullerenes and nanotubes. However, it has not been tested for the case of functionalized fullerenes (especially with highly strained geometries). We use the Brenner potential for our companion nanogear simulations and believe that it should be calibrated to insure that those simulations are physically reasonable. In the present work, Density Functional theory (DFT) calculations are used to determine the preferred geometric structures and energetics for this calibration. The DFT method is a kind of ab initio quantum chemistry method for determining the electronic structure of molecules. For a given basis set expansion, it is comparable in accuracy to the MP2 method (better than Hartree Fock, but less accurate than more extensive electron correlation methods such as MP4 or CCSD). However, for systems with large numbers of basis functions it more efficient than any other methods that include electron correlation effects. In this presentation we show the results of DFT calculations for the reaction of benzyne with naphthalene, C60, and nanotube models. We compare energies for [2+2] and [2+4] cycloaddition products. The preferred products for the naphthalene and C60 reactions have been determined by experiment and, thus, these cases serve as a validation of our quantum chemical approach. We also compare the DFT and Brenner potential results. Finally we can predict the likelihood of reaction between benzyne and nanotubes.
Jaffe, Richard↗
Quantum Chemistry Study of Cycloaddition Pathways for the Reaction of o-Benzyne with Fullerenes and Carbon Nanotubes
Functionalization of fullerenes via the [2+2] cycloaddition reaction with o-benzyne has been demonstrated in the laboratory. In contrast, [2+4) cycloaddition products are formed when benzyne reacts with planar polycyclic aromatic hydrocarbons. Using density functional theory (DFT) calculations with Becke's hybrid functional and small contracted gaussian basis sets, we are able to reproduce these product preferences. The objective of this work is to explore the functionalization of carbon nanotubes. We have studied o-benzyne cycloaddition products with a [14,0] single-walled nanotube. We find both the [2+2] and [2+4] adducts to be stable, with the latter product being somewhat favored.
Jaffe, Richard↗
Photoionization of Benzene and Small Polycyclic Aromatic Hydrocarbons in Ultraviolet-Processed Astrophysical Ices: A Computational Study
We employed density functional theory (DFT) calculations to model the photoionization behavior of benzene and small polycyclic aromatic hydrocarbons when they are embedded in a matrix of water ice in order to investigate issues raised by recent experimental work by Gudipati and Allamandola. The ionization energies of benzene, naphthalene, anthracene, and pyrene were found to be lowered by 1.5-2.1 eV in water ice. Low-lying vertical electronic excitation energies were computed with time-dependent DFT for both neutral and ionized species and are found in both cases to be remarkably unaffected by the ice matrix. Chemical behavior in ultraviolet-photoprocessed ices is also discussed, with a focus on electron recombination and pathways leading to phenol and analogous products.
Woon, D. E.↗
Theoretical Investigation of OCN(-) Charge Transfer Complexes in Condensed Phase Media: Spectroscopic Properties in Amorphous Ice
Density functional theory (DFT) calculations of cyanate (OCN(-)) charge-transfer complexes were performed to model the "XCN" feature observed in interstellar icy grain mantles. OCN(-) charge-transfer complexes were formed from precursor combinations of HNCO or HOCN with either NH3 or H2O. Three different solvation strategies for realistically modeling the ice matrix environment were explored, including (1) continuum solvation, (2) pure DFT cluster calculations, and (3) an ONIOM DFT/PM3 cluster calculation. The model complexes were evaluated by their ability to reproduce seven spectroscopic measurements associated with XCN: the band origin of the OCN(-) asymmetric stretching mode, shifts in that frequency due to isotopic substitutions of C, N, O, and H, plus two weak features. The continuum solvent field method produced results consistent with some of the experimental data but failed to account for other behavior due to its limited capacity to describe molecular interactions with solvent. DFT cluster calculations successfully reproduced the available spectroscopic measurements very well. In particular, the deuterium shift showed excellent agreement in complexes where OCN(-) was fully solvated. Detailed studies of representative complexes including from two to twelve water molecules allowed the exploration of various possible solvation structures and provided insights into solvation trends. Moreover, complexes arising from cyanic or isocyanic acid in pure water suggested an alternative mechanism for the formation of OCN(-) charge-transfer complexes without the need for a strong base such as NH3 to be present. An extended ONIOM (B3LYP/PM3) cluster calculation was also performed to assess the impact of a more realistic environment on HNCO dissociation in pure water.
Park, Jin-Young↗
Theoretical Modeling of Formic Acid (HCOOH), Formate (HCOO(-)), and Ammonia (NH(4)) Vibrational Spectra in Astrophysical Ices
Ions embedded in icy grain mantles are thought to account for various observed infrared spectroscopic features, particularly in certain young stellar objects. The dissociation of formic acid (HCOOH) in astrophysical ices to form the formate ion (HCOO(-)) was modeled with density functional theory cluster calculations. Like isocyanic acid (HOCN), HCOOH was found to spontaneously deprotonate when sufficient water is present to stabilize charge transfer complexes. Both ammonia and water can serve as proton acceptors, yielding ammonium (NH4(+)) and hydronium (H3O(+)) counterions. Computed frequencies of weak infrared features produced by stretching and bending modes in both HCOO(-) and HCOOH were compared with experimental and astronomical data. Our results confirm laboratory assignments that a band at 1381 cm(exp -1) can be attributed to the CH bend in either HCOO(-) or HCOOH, but a band at 1349 cm(exp -1) corresponds to CO stretching in HCOO(-). Another feature at 1710 cm(exp -1) (5.85 m) can possibly be assigned to a CO stretching mode in HCOOH, as suggested by experiment, but the agreement is less satisfactory. In addition, we examine and analyze spectroscopic features associated with NH+4, both as a counterion to HCOO(-) or OCN(-) and in isolation, in order to compare with experimental and astronomical data in the 7 m region.
Park, Jin-Young↗
Ab initio Computations of the Electronic, Mechanical, and Thermal Properties of Ultra High Temperature Ceramics (UHTC) ZrB2 and HfB2
Refractory materials such as metallic borides, often considered as ultra high temperature ceramics (UHTC), are characterized by high melting point, high hardness, and good chemical inertness. These materials have many applications which require high temperature materials that can operate with no or limited oxidation. Ab initio, first principles methods are the most accurate modeling approaches available and represent a parameter free description of the material based on the quantum mechanical equations. Using these methods, many of the intrinsic properties of these material can be obtained. We performed ab initio calculations based on density functional theory for the UHTC materials ZrB2 and HfB2. Computational results are presented for structural information (lattice constants, bond lengths, etc), electronic structure (bonding motifs, densities of states, band structure, etc), thermal quantities (phonon spectra, phonon densities of states, specific heat), as well as information about point defects such as vacancy and antisite formation energies.
Lawson, John W.↗
Aladyn - Adaptive Neural Network Molecular Dynamics Simulation Code: Computational Materials Mini-Application
This report provides an overview and commands description of the Computational Materials mini-application, Aladyn. Aladyn is a simple molecular dynamics code written in FORTRAN 2008, which is designed to demonstrate the use of adaptive neural networks (ANNs) in atomistic simulations. The role of ANNs is to reproduce the very complex energy landscape resulting from the atomic interactions in materials with the accuracy of quantum mechanics-based energy calculations. The ANN is trained on a large set of atomic structures calculated using the density functional theory (DFT) method. The Aladyn code is being released to serve as a training testbed for students and professors in academia to explore possible optimization algorithms for parallel computing on multicore central processing unit (CPU) computers or computers utilizing many core architectures based on graphic processing units (GPUs). The effort is related to the High Performance Computing Incubator (HPCI) project at NASA Langley Research Center.
Yamakov, Vesselin I.↗
Cavity Ring-Down Spectroscopy of Anthracene, 9-Methylanthracene, and 2 Methylanthracene in Supersonic Expansion
The S0–S1 absorption spectra of anthracene (C14H10), 9-methylanthracene (C15H12), and 2-methylanthracene (C15H12) are measured in the ultraviolet region between 330 and 375 nm (26,666 to 30,303 cm–1) with cavity ring-down spectroscopy in supersonic free-jet expansions of argon. The associated vibronic band systems and their spectroscopic assignments are discussed and compared to previous studies performed using fluorescence excitation and dispersed fluorescence techniques. Density functional theory (DFT) calculations were carried out to study the structures and evaluate the vibrational transitions of the ground and excited states. Time-dependent DFT calculations of the first electronic excited states and Franck–Condon factor calculations were carried out to assist in the assignment of the experimentally measured vibronic bands. The vibronic spectra obtained in absorption agree well with fluorescence excitation spectra in terms of peak positions but exhibit different relative band intensities. We find a very good match between experimentally obtained vibronic line positions and the peak positions of the quantum chemically calculated Franck–Condon excitation lines.
Salma Bejaoui↗
Galactic Cosmic Ray Event-Based Risk Model (GERM) Code
This software describes the transport and energy deposition of the passage of galactic cosmic rays in astronaut tissues during space travel, or heavy ion beams in patients in cancer therapy. Space radiation risk is a probability distribution, and time-dependent biological events must be accounted for physical description of space radiation transport in tissues and cells. A stochastic model can calculate the probability density directly without unverified assumptions about shape of probability density function. The prior art of transport codes calculates the average flux and dose of particles behind spacecraft and tissue shielding. Because of the signaling times for activation and relaxation in the cell and tissue, transport code must describe temporal and microspatial density of functions to correlate DNA and oxidative damage with non-targeted effects of signals, bystander, etc. These are absolutely ignored or impossible in the prior art. The GERM code provides scientists data interpretation of experiments; modeling of beam line, shielding of target samples, and sample holders; and estimation of basic physical and biological outputs of their experiments. For mono-energetic ion beams, basic physical and biological properties are calculated for a selected ion type, such as kinetic energy, mass, charge number, absorbed dose, or fluence. Evaluated quantities are linear energy transfer (LET), range (R), absorption and fragmentation cross-sections, and the probability of nuclear interactions after 1 or 5 cm of water equivalent material. In addition, a set of biophysical properties is evaluated, such as the Poisson distribution for a specified cellular area, cell survival curves, and DNA damage yields per cell. Also, the GERM code calculates the radiation transport of the beam line for either a fixed number of user-specified depths or at multiple positions along the Bragg curve of the particle in a selected material. The GERM code makes the numerical estimates of basic physical and biophysical quantities of high-energy protons and heavy ions that have been studied at the NASA Space Radiation Laboratory (NSRL) for the purpose of simulating space radiation biological effects. In the first option, properties of monoenergetic beams are treated. In the second option, the transport of beams in different materials is treated. Similar biophysical properties as in the first option are evaluated for the primary ion and its secondary particles. Additional properties related to the nuclear fragmentation of the beam are evaluated. The GERM code is a computationally efficient Monte-Carlo heavy-ion-beam model. It includes accurate models of LET, range, residual energy, and straggling, and the quantum multiple scattering fragmentation (QMSGRG) nuclear database.
Cucinotta, Francis A.↗
Simplified model of statistically stationary spacecraft rotation and associated induced gravity environments
A stochastic model of spacecraft motion was developed based on the assumption that the net torque vector due to crew activity and rocket thruster firings is a statistically stationary Gaussian vector process. The process had zero ensemble mean value, and the components of the torque vector were mutually stochastically independent. The linearized rigid-body equations of motion were used to derive the autospectral density functions of the components of the spacecraft rotation vector. The cross-spectral density functions of the components of the rotation vector vanish for all frequencies so that the components of rotation were mutually stochastically independent. The autospectral and cross-spectral density functions of the induced gravity environment imparted to scientific apparatus rigidly attached to the spacecraft were calculated from the rotation rate spectral density functions via linearized inertial frame to body-fixed principal axis frame transformation formulae. The induced gravity process was a Gaussian one with zero mean value. Transformation formulae were used to rotate the principal axis body-fixed frame to which the rotation rate and induced gravity vector were referred to a body-fixed frame in which the components of the induced gravity vector were stochastically independent. Rice's theory of exceedances was used to calculate expected exceedance rates of the components of the rotation and induced gravity vector processes.
Fichtl, G. H.↗
Density sensitive X-ray line ratios in the Be I, B I, and Ne I isoelectronic sequences
The intensities of X-ray transitions in highly charged ions in the Be I, B I, and Ne I isoelectronic sequences have been calculated as functions of electron density. The intensities of the transitions from the 2s(n)2p(m)3p configuration, relative to the intensities from the 2s(n)2p(m)3s and 2s(n)p(m)3d configurations, are strong functions of electron density in high-density plasmas. The density sensitivity occurs at electron densities between 10 to the 16th/cu cm (for Si ions) and 10 to the 22nd/cu cm (for Kr ions). Opacity is unimportant for plasma dimensions that are characteristic of dense laser-produced plasmas. These X-ray line ratios represent a promising new density diagnostic for high-density plasmas.
Feldman, U.↗
Pressure algorithm for elliptic flow calculations with the PDF method
An algorithm to determine the mean pressure field for elliptic flow calculations with the probability density function (PDF) method is developed and applied. The PDF method is a most promising approach for the computation of turbulent reacting flows. Previous computations of elliptic flows with the method were in conjunction with conventional finite volume based calculations that provided the mean pressure field. The algorithm developed and described here permits the mean pressure field to be determined within the PDF calculations. The PDF method incorporating the pressure algorithm is applied to the flow past a backward-facing step. The results are in good agreement with data for the reattachment length, mean velocities, and turbulence quantities including triple correlations.
Anand, M. S.↗
Extragalactic Backgrounds in the Far UV and Exploring Star Formation at High Redshifts with Gamma-ray Observations
The determination of the intergalactic photon densities from the FIR to the UV which is produced by stellar emission and dust reradiation at various redshifts can provide an independent measure of the star formation history of the universe. Using recent Spitzer and GALEX data in conjunction with other observational inputs, Stecker, Malkan and Scully have calculated the intergalactic photon density as a function of both energy and redshift for 0 < zeta < 6 for photon energies from 0.003 eV to the Lyman limit cutoff at 13.6 eV in a ACDM universe with Omega(sub Lambda) = 0.7 and Omega(sub m) = 0.3. Their results are based on backwards evolution models for galaxies which were developed by Malkan and Stecker previously. The calculated background SEDs at zeta = 0 are in good agreement with the present observational data and limits. The calculated intergalactic photon densities as a function of redshift were used to predict to extend the absorption of high energy 7-rays in intergalactic space from sources such as blazars and quasars, this absorption being produced by interactions the y-rays with the intergalactic FIR-UV photons having the calculated densities. The results are in excellent agreement with absorption features found in the low gamma-ray spectra of Mkn 421, Mkn 501 at, zeta = 0.03 and PKS
Stecker, Floyd W.↗
Calculated nighttime eastward plasma drift velocities at low latitudes and their solar cycle dependence
After calculating ambient electron densities as a function of altitude, latitude and local time, a simplified expression is used to calculate F-region eastward plasma drifts given a zonal neutral wind model. The derived eastward plasma drift on a magnetic flux tube is examined as a function of the flux tube apex height. If the neutral wind is assumed to be independent of latitude the plasma drift maximizes along the flux tube which intercepts the F-region peak concentration at the Appleton anomaly. Above this altitude the velocity decreases to reflect a decrease in the flux tube integrated F-region Pedersen conductivity. For a latitude dependent wind the plasma drift tends to maximize along the flux tube which intercepts the F-peak at the dip equator. Above this altitude the drift decreases to reflect the latitude distribution of the wind.
Anderson, D. N.↗
Molecular dissociation and shock-induced cooling in fluid nitrogen at high densities and temperatures
Radiative temperatures and electrical conductivities were measured for fluid nitrogen compressed dynamically to pressures of 18-90 GPa, temperatures of 4000-14,000 K, and densities of 2-3 g/cu cm. The data show a continuous phase transition above 30 GPa shock pressure and confirm that (delta-P/delta-T)v is less than 0, as indicated previously by Hugoniot equation-of-state experiments. The first observation of shock-induced cooling is also reported. The data are interpreted in terms of molecular dissociation, and the concentration of dissociated molecules is calculated as a function of density and temperature.
Radousky, H. B.↗
Imperfection surveys on a 10-ft-diameter shell structure
The results of an extensive imperfection survey on a 10-ft-diameter integrally stiffened cylindrical shell are presented. The shape of the measured initial imperfections is clearly influenced by details of the shell construction. The modal components of the measured imperfection surface as a function of the circumferential and of the axial wave numbers are calculated. The discrete axial power spectral density functions and the corresponding root-mean-square values of the imperfections are also determined for given circumferential wave numbers. Using the Fourier coefficients of the measured initial imperfections, buckling loads are calculated by solving the nonlinear Donnell-type imperfect shell equations iteratively. The calculated lowest buckling load compares favorably with the values usually recommended for similar shell structures.
Arbocz, J.↗